US3362983A - Process for the manufacture of ethylenes substituted in the 1-position - Google Patents

Process for the manufacture of ethylenes substituted in the 1-position Download PDF

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Publication number
US3362983A
US3362983A US377413A US37741364A US3362983A US 3362983 A US3362983 A US 3362983A US 377413 A US377413 A US 377413A US 37741364 A US37741364 A US 37741364A US 3362983 A US3362983 A US 3362983A
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United States
Prior art keywords
cyclobutane
cleavage
temperature
group
substituted
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Expired - Lifetime
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US377413A
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English (en)
Inventor
Sennewald Kurt
Vogt Wilhelm
Erpenbach Heinz
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Knapsack AG
Knapsack Griesheim AG
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Knapsack AG
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    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C253/00Preparation of carboxylic acid nitriles
    • C07C253/30Preparation of carboxylic acid nitriles by reactions not involving the formation of cyano groups
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B29WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29CSHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
    • B29C33/00Moulds or cores; Details thereof or accessories therefor
    • B29C33/56Coatings, e.g. enameled or galvanised; Releasing, lubricating or separating agents
    • B29C33/60Releasing, lubricating or separating agents
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C209/00Preparation of compounds containing amino groups bound to a carbon skeleton
    • C07C209/68Preparation of compounds containing amino groups bound to a carbon skeleton from amines, by reactions not involving amino groups, e.g. reduction of unsaturated amines, aromatisation, or substitution of the carbon skeleton
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C51/00Preparation of carboxylic acids or their salts, halides or anhydrides
    • C07C51/347Preparation of carboxylic acids or their salts, halides or anhydrides by reactions not involving formation of carboxyl groups
    • C07C51/353Preparation of carboxylic acids or their salts, halides or anhydrides by reactions not involving formation of carboxyl groups by isomerisation; by change of size of the carbon skeleton
    • CCHEMISTRY; METALLURGY
    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09BORGANIC DYES OR CLOSELY-RELATED COMPOUNDS FOR PRODUCING DYES, e.g. PIGMENTS; MORDANTS; LAKES
    • C09B23/00Methine or polymethine dyes, e.g. cyanine dyes
    • C09B23/02Methine or polymethine dyes, e.g. cyanine dyes the polymethine chain containing an odd number of >CH- or >C[alkyl]- groups
    • C09B23/04Methine or polymethine dyes, e.g. cyanine dyes the polymethine chain containing an odd number of >CH- or >C[alkyl]- groups one >CH- group, e.g. cyanines, isocyanines, pseudocyanines

Definitions

  • the present invention is concerned with a process for the manufacture of ethylenes which are substituted in the l-position and have the general formula:
  • R stands for either a hydrogen atom or a halogenatom, and R stands for a carboxylic acid group, an ester group or nitrile group or an aminomethyl'group, by thermal cleavage to cyclobutane compounds having corresponding substituents in the 1,2-position.
  • cis-1,2-dimethylcyclobutane can be subjected to thermal cleavage under reduced pressure at a temperature of 380 to 430 0, resulting in the formation of cleavage products consisting partially of propylene and ethylene and a mixture comprising cis-2-butene and trans2-butene.
  • the nature of the isolated cleavage products indicates that cis-1,2-dimethylcyclobutane is split at high temperatures in both the 1,2- and 3,4-linkages and in the 2,3- and 1,4-linkages.
  • the present invention unexpectedly provides a process for making ethylenes substituted in the 1-position, wherein a compound having the general formula:
  • R stands for either a hydrogen atom or a halogen atom and R stands for a carboxylic group, an ester group or a nitrile group, or in which R stands for a hydrogen atom and R stands for a CH -NH group
  • R stands for either a hydrogen atom or a halogen atom and R stands for a carboxylic group, an ester group or a nitrile group, or in which R stands for a hydrogen atom and R stands for a CH -NH group
  • R stands for a hydrogen atom and R stands for a CH -NH group
  • R1 CH2 C/ R2 in which R stands for a hydrogen atom or a halogen atom and R stands for a carboxylic group, an ester group or a nitrile group, or R stands for a hydrogen atom and R stands for a -CH -NH group.
  • the starting materials suitable for use in the process of the present invention include, for example: cyclobutane-1,2-dicarboxylic acid or 1,2dihalogeno-, e.g. 1,2-dichloroor 1,2-dibromo-cyclobutane-1,2-dicarboxylic acid, or the methyl-, ethyl, propyl or butyl ester of cyclobutane-1,2-dicarboxylic acid and the corresponding esters of 1,2-dihalogeno-, e.g.
  • 1,Z-dihalogeno-cyclobutane compounds there may also be used l-halogeno-cyclobutane compounds, eg, l-halogeno-cyclobutane-1,2-dinitrile, 1- halogeno-cyclobutane-1,2-dicarboxylic acid and esters of l-halogeno-cyclobutane-1,2-dicarboxylic acid, the alcoholic components of which have 1 to 4 carbon atoms.
  • chlorine or bromine derivatives of cyclobutane are used as the halogenated starting products.
  • the above starting products are thermally split by being passed in vapor form through e.g. an electrically heated quartz tube, which is preferably maintained at a temperature of about 600 to 700 C. and under a pressure of preferably 5 to 20 mm. mercury.
  • the vapors are allowed to remain in the reaction tube for a period of time of preferably about 0.5 to 2 seconds.
  • the cleavage gas leaving the reaction tube should be cooled in a condenser at a temperature of about 20 to 30 C. and thereafter be liquefied and collected in a receiver cooled at a tempera ture of e.g. C.
  • the liquefied cleavage product is distilled in conventional manner.
  • the products prepared by the process of the present invention are mostly obtained in yields of more than They deserve special commercial interest because they are used inter alia as starting material for numerous syntheses and as monomers for use in polymerization and copolymerization processes.
  • the small losses in yield are 3 not the result of a cleavage reaction other than in the 1,2- and 3,4-linkages, but are the customary result of the finishing treatment to which the products are ultimately subjected.
  • Example 1 146 grams 1,2-dichloro-cyclobutane-1,2-dinitrile were 'caused to flow in vapor form at a pressure of 12 mm.
  • Example 3 172 grams cyclobutane-1,2-dicarboxy1ic acid dimethylester, which had been obtained by hydrolyzing cyclobutane-LZdinitrile followed by esterification with methanol, were split in an electrically heated quartz tube at a pressure of 10 mm. mercury, a temperature of 600 C. and a time of residence of the material in the tube of 0.1 second. The resulting cleavage product and unreacted ester were separated by means of a condenser and collected in a receiver cooled at 70 C. The condensed reaction mixture was separated into its components by fractional distillation resulting in the formation of 72 grams acrylic acid methylester having a B.P. of 40-41 C. and of 93 grams unreacted ester. 45% of the cyclobutane-1,2-dicanboxylic acid dimethylester underwent conversion, and the acrylic acid methylester was obtained in a yield of 91.3%.
  • Example 4 Cyclobutane-l,Z-dicarboxylic acid dibutylester, prepared by hydrolyzing cyclobutane-1,2-dinitrile followed by esterification with butanol, was split in a quartz tube at a pressure of 30 mm. mercury,.a temperature of 650 C. and a residence time of 0.1 second of the compound in the tube. Fractional distillation of the reaction mixture indicated a conversion rate of 78.4%, and acrylic acid butylester was obtained in a yield of 52.1% of the theoretical.
  • Example 5 1 chloro cyclobutane-1,2-dicarboxylic dimethylester was split in the gaseous phase in a manner, analogous to that described in the preceding examples at 700 C., a pressure of mm. mercury and a time of residence of 0.11 second. The conversion rate was 92.1%. a-chloroacrylic acid methylester (B.P. :58 C.) and acrylic acid methylester were obtained in equal parts in a yield of 677.8% of the theoretical.
  • Example 6 1,2-dichloro-cyclobutane-1,Z-dicarboxylic acid dimethylester was split under the conditions set forth in Example tuted in the 1-position, consisting essentially in passing a 4 5. The conversion rate was 88.4%, and a-chloro-acrylic acid methylester was obtained in a yield of 64% of the theoretical.
  • Example 7 216 grams cyclobutane-1,2-dicarboxylic acid were caused to flow in vapor form at a pressure of 25 mm. mercury and at a temperature of 600 C. through an electrically heated quartz tube, and thermally split therein.
  • the vapors were allowed to remain in the quartz tube for 0.13 second.
  • the cleavage gases flowing oil were condensed and collected in a receiver cooled at -70 C..

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Engineering & Computer Science (AREA)
  • Mechanical Engineering (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
US377413A 1963-07-12 1964-06-23 Process for the manufacture of ethylenes substituted in the 1-position Expired - Lifetime US3362983A (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DEK50201A DE1238899B (de) 1963-07-12 1963-07-12 Verfahren zur Herstellung von alpha-Halogenacryl-saeureestern oder -nitrilen
DEK50786A DE1230014B (de) 1963-07-12 1963-09-10 Verfahren zur Herstellung von primaerem Allylamin

Publications (1)

Publication Number Publication Date
US3362983A true US3362983A (en) 1968-01-09

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US377413A Expired - Lifetime US3362983A (en) 1963-07-12 1964-06-23 Process for the manufacture of ethylenes substituted in the 1-position

Country Status (7)

Country Link
US (1) US3362983A (de)
AT (1) AT252198B (de)
BE (2) BE650379A (de)
CH (1) CH433250A (de)
DE (2) DE1238899B (de)
GB (1) GB1043305A (de)
NL (1) NL142943B (de)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3507902A (en) * 1967-07-21 1970-04-21 Standard Oil Co Process for preparing alpha-chloroacrylonitriles

Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2773089A (en) * 1954-10-29 1956-12-04 Du Pont Fluorinated olefinic nitriles
US3092654A (en) * 1960-06-17 1963-06-04 Du Pont Preparation of dicarboxylic acid nitriles

Family Cites Families (16)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR1317753A (de) * 1963-05-08
US2673875A (en) * 1950-10-11 1954-03-30 Gen Aniline & Film Corp Dehydrohalogenation of dihalopropionic acid compounds
GB723547A (en) * 1951-12-31 1955-02-09 Distillers Co Yeast Ltd Esters and nitriles of alphahaloacrylic acids
GB750638A (en) * 1953-01-21 1956-06-20 Gen Aniline & Film Corp Dehydrochlorination of dichloropropionic acid compounds
GB813175A (en) * 1954-08-06 1959-05-13 Charles Herschmann Process for the production of monohalogenated vinyl compounds from ª‡,ª‰-dihalogenated compounds
DE1030332B (de) * 1955-11-09 1958-05-22 Basf Ag Verfahren zur Herstellung von ª‡-Chloracrylsaeureestern
DE1064502B (de) * 1956-03-01 1959-09-03 Basf Ag Verfahren zur Herstellung von alpha-Chloracrylsaeureestern aus Dichlorpriopionsaeureern durch Chlorwasserstoffabspaltung
DE1024956B (de) * 1956-03-01 1958-02-27 Basf Ag Verfahren zur Herstellung von ª‡-Chloracrylsaeureestern aus Dichlorpropionsaeureestern durch Chlorwasserstoffabspaltung
DE1021357B (de) * 1956-03-01 1957-12-27 Basf Ag Verfahren zur Herstellung von ª‡-Chloracrylsaeureestern aus Dichlorpropionsaeureestern durch Chlorwasserstoffabspaltung
DE1076673B (de) * 1956-03-01 1960-03-03 Basf Ag Verfahren zur Herstellung von ª‡-Chloracrylsaeureestern aus Dichlorpropionsaeureestern durch Chlorwasserstoffabspaltung
DE1030333B (de) * 1956-05-08 1958-05-22 Basf Ag Verfahren zur Herstellung von ª‡-Chloracrylsaeureestern
US2870193A (en) * 1957-03-15 1959-01-20 Maxwell A Pollack Making alpha-chloroacrylic compounds
DE1089754B (de) * 1959-10-24 1960-09-29 Knapsack Ag Verfahren zur Herstellung von 1, 2-Dicyancyclobutan
DE1081008B (de) * 1959-02-06 1960-05-05 Knapsack Ag Verfahren zur Herstellung von 1, 2-Dicyancyclobutan
DE1103330B (de) * 1960-01-23 1961-03-30 Knapsack Ag Verfahren zur Herstellung von 1, 2-Dicyancyclobutan
DE1150381B (de) * 1961-02-22 1963-06-20 Muenzing & Comp Chem Fab Verfahren zur Herstellung von ª‡-Chloracrylsaeurenitril durch Abspaltung von Chlorwasserstoff aus ª‡, ª‰-Dichlorpropionsaeurenitril

Patent Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2773089A (en) * 1954-10-29 1956-12-04 Du Pont Fluorinated olefinic nitriles
US3092654A (en) * 1960-06-17 1963-06-04 Du Pont Preparation of dicarboxylic acid nitriles

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3507902A (en) * 1967-07-21 1970-04-21 Standard Oil Co Process for preparing alpha-chloroacrylonitriles

Also Published As

Publication number Publication date
DE1238899B (de) 1967-04-20
GB1043305A (en) 1966-09-21
NL142943B (nl) 1974-08-15
CH433250A (de) 1967-04-15
BE650455A (de)
AT252198B (de) 1967-02-10
NL6407892A (de) 1965-01-13
DE1230014B (de) 1966-12-08
BE650379A (de) 1964-11-03

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